Hierarchical pore configuration in activated coke boosting direct desorption of desulfurization product H2SO4: A combined experimental and computational investigation
Hierarchical pore configuration in activated coke boosting direct desorption of desulfurization product H2SO4: A combined experimental and computational investigation
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活性焦中的分级孔隙结构促进脱硫产物 H2SO4 的直接解吸：实验和计算相结合的研究
DOI：
10.1016/j.fuel.2021.120697
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发表时间：
2021-08
期刊：
影响因子：
7.4
通讯作者：
Gao Jihui
中科院分区：
文献类型：
--
作者：
Pi Xinxin;Sun Fei;Qu Zhibin;Li Yang;Gao Jihui
水洗再生已应用于从脱硫活性焦（AC）中回收H2SO4。然而，再生效率低是导致活性炭循环脱硫性能较差的瓶颈。在此，我们提出通过AC的孔结构调节可以显着提高洗涤再生效率。使用一系列具有可变孔结构的活性炭作为模型吸附剂，单独研究孔结构对脱硫活性炭洗涤再生的影响。循环脱硫-再生实验表明，微孔活性炭的水洗再生性能较差。经过10次循环后，微孔活性炭的吸附硫容量下降至10.17 mg g−1，仅为新鲜活性焦的50%。而含有等量微孔和中孔体积（0.40和0.50 cm3g−1）的分级多孔活性炭同时具有优异的SO2去除动力学和水洗再生性能。即使经过10次循环，分级多孔活性炭仍能保持70 mg g−1的高吸附硫容量和90%的优异水洗再生效率。采用接近实际AC的孔隙模型进行分子动力学模拟表明，分级孔隙中H2SO4的自扩散系数约为微孔中的2倍，证明了分级多孔结构对H2SO4解吸的促进作用。这项工作不仅揭示了孔隙构型与洗涤再生行为的关系，而且提供了一种简便的孔隙构型调控策略，可以显着提高活性炭的再生效率，意味着水洗再生在工业脱硫过程中应用的巨大潜力。
Water washing regeneration has been applied to recover H2SO4from desulfurized activated cokes (AC). However, the low regeneration efficiency is the bottleneck which causes inferior cycled desulfurization properties of AC. Herein, we propose that the washing regeneration efficiency can be significantly improved by pore structure regulation of AC. A series of ACs with variable pore configurations were used as model adsorbents to individually investigate the effect of pore structure on the washing-regeneration of desulfurized AC. Cycling desulfurization-regeneration experiments show that the micropore-dominant AC exhibits poor performance of water-washing regeneration. After 10 cycles, the adsorption sulfur capacity of micropore-dominant AC declines to 10.17 mg g−1, only 50% of fresh activated coke. Whereas the hierarchical porous AC containing equivalent volume of micropore and mesopore (0.40 and 0.50 cm3g−1) has both excellent SO2removal kinetics and water-washing regeneration performance. Even after 10 cycles, the hierarchical porous AC can still sustain high adsorption sulfur capacity of 70 mg g−1and excellent water-washing regeneration efficiency of 90%. Molecular dynamic simulations using pore models close to practical AC suggest that the self-diffusion coefficient of H2SO4in hierarchical pore is about two times of that in micropore, proving the promoting role of hierarchical porous structure in H2SO4desorption. This work not only reveals the relationship of pore configuration with washing regeneration behavior but also provides a facile pore configuration regulation strategy that can substantially improve AC’s regeneration efficiency, implying great potentials for applying water-washing regeneration in industrial desulfurization process.
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影响因子：
8.6
作者：
Tamar Zelovich;Leslie Vogt-Maranto;M. Hickner;S. Paddison;Chulsung Bae;Dario R. Dekel;M. Tuckerman
通讯作者：
Tamar Zelovich;Leslie Vogt-Maranto;M. Hickner;S. Paddison;Chulsung Bae;Dario R. Dekel;M. Tuckerman
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影响因子：
5.3
作者：
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通讯作者：
Jin Yan
影响因子：
5.3
作者：
I. Mochida;S. Miyamoto;Keiichi Kuroda;S. Kawano;S. Yatsunami;Y. Korai;A. Yasutake;M. Yoshikawa
通讯作者：
I. Mochida;S. Miyamoto;Keiichi Kuroda;S. Kawano;S. Yatsunami;Y. Korai;A. Yasutake;M. Yoshikawa
影响因子：
3.3
作者：
Liu, Bo;Wu, Renbing;Zhou, Kun
通讯作者：
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影响因子：
15.1
作者：
Rosas, Juana M.;Ruiz-Rosas, Ramiro;Cordero, Tomas
通讯作者：
Cordero, Tomas